Hyper-Rayleigh scattering and hyper-Raman scattering of dye-adsorbed silver nanoparticles induced by a focused continuous-wave near-infrared laser

We report that hyper-Rayleigh scattering, surface-enhanced hyper-Raman scattering, and two-photon excited luminescence occur intermittently by focusing a continuous-wave near-infrared (cw-NIR) laser into a colloidal silver solution including rhodamine 6G (R6G) and sodium chloride (NaCl). On the other hand, continuous hyper-Rayleigh scattering is observed from colloidal silver free from R6G and NaCl, demonstrating that hyper-Raman scattering and two-photon excited luminescence are attributed to R6G and their intermittent features are dependent on the colloidal dispersion. These results suggest that the cw-NIR laser has three roles; the source of the nonlinear response, optical trapping of nanoparticles, and making nanoparticle aggregates possessing the high activity for the nonlinear response.